Metal-mediated self-assembly of supramolecular assemblies has been proven to be an efficient tool for developing new materials with well-defined shapes and geometries. Among this, banana-shaped bis-monodentate ligands react with Pd(II) cations to a broad range of topologies from small Pd2L4 cages, their interpenetrated dimers, rings of various size up to large Pd24L48 spheres. We embed functions into supramolecular cages, for example allosteric guest binding or light-responsive behaviour. However, most of the reported examples are highly symmetric structures carrying only one functionality. Previously we included two different functionalities, donor and acceptor moieties that undergo light-induced charge separation, within interpenetrated double cages (Figure a). However, this system suffers from a lack of control over stoichiometry and stereochemistry. Recently we started to develop rational design strategies to assemble heteroleptic cages in a non-statistical fashion. We successfully used donor site engineering (Figure b,c), geometric shape complementarity (Figure d), and ring-embedded-metal approaches to obtain integrative self-sorting of multicomponent cages. Currently we are studying emerging properties based on the interactions of at least two functionalities.

Self-assembly strategies for multifunctional and stimuli-responsive coordination cages

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

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